Analysis of sensitivity enhancement by ...
Document type :
Article dans une revue scientifique: Article original
DOI :
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Title :
Analysis of sensitivity enhancement by dynamic nuclear polarization in solid-state NMR: a case study of functionalized mesoporous materials
Author(s) :
Kobayashi, Takeshi [Auteur]
Lafon, Olivier [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Lilly Thankamony, Aany S. [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Slowing, Igor I. [Auteur]
Kandel, Kapil [Auteur]
Carnevale, Diego [Auteur]
Vitzthum, Veronika [Auteur]
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Amoureux, Jean-Paul [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Bodenhausen, Geoffrey [Auteur]
Pruski, Marek [Auteur]
Lafon, Olivier [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Lilly Thankamony, Aany S. [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Slowing, Igor I. [Auteur]
Kandel, Kapil [Auteur]
Carnevale, Diego [Auteur]
Vitzthum, Veronika [Auteur]
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Amoureux, Jean-Paul [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Bodenhausen, Geoffrey [Auteur]
Pruski, Marek [Auteur]
Journal title :
Physical Chemistry Chemical Physics
Abbreviated title :
Phys. Chem. Chem. Phys.
Volume number :
15
Pages :
5553
Publisher :
Royal Society of Chemistry (RSC)
Publication date :
2013-02-01
ISSN :
1463-9076
HAL domain(s) :
Chimie/Chimie théorique et/ou physique
Chimie/Chimie organique
Chimie/Chimie organique
English abstract : [en]
We systematically studied the enhancement factor (per scan) and the sensitivity enhancement (per unit time) in 13C and 29Si cross-polarization magic angle spinning (CP-MAS) NMR boosted by dynamic nuclear polarization (DNP) ...
Show more >We systematically studied the enhancement factor (per scan) and the sensitivity enhancement (per unit time) in 13C and 29Si cross-polarization magic angle spinning (CP-MAS) NMR boosted by dynamic nuclear polarization (DNP) of functionalized mesoporous silica nanoparticles (MSNs). Specifically, we separated contributions due to: (i) microwave irradiation, (ii) quenching by paramagnetic effects, (iii) the presence of frozen solvent, (iv) the temperature, as well as changes in (v) relaxation and (vi) cross-polarization behaviour. No line-broadening effects were observed for MSNs when lowering the temperature from 300 to 100 K. Notwithstanding a significant signal reduction due to quenching by TOTAPOL radicals, DNP-CP-MAS at 100 K provided global sensitivity enhancements of 23 and 45 for 13C and 29Si, respectively, relative to standard CP-MAS measurements at room temperature. The effects of DNP were also ascertained by comparing with state-of-the-art two-dimensional heteronuclear 1H{13C} and 29Si{1H} correlation spectra, using, respectively, indirect detection or Carr–Purcell–Meiboom–Gill (CPMG) refocusing to boost signal acquisition. This study highlights opportunities for further improvements through the development of high-field DNP, better polarizing agents, and improved capabilities for low-temperature MAS.Show less >
Show more >We systematically studied the enhancement factor (per scan) and the sensitivity enhancement (per unit time) in 13C and 29Si cross-polarization magic angle spinning (CP-MAS) NMR boosted by dynamic nuclear polarization (DNP) of functionalized mesoporous silica nanoparticles (MSNs). Specifically, we separated contributions due to: (i) microwave irradiation, (ii) quenching by paramagnetic effects, (iii) the presence of frozen solvent, (iv) the temperature, as well as changes in (v) relaxation and (vi) cross-polarization behaviour. No line-broadening effects were observed for MSNs when lowering the temperature from 300 to 100 K. Notwithstanding a significant signal reduction due to quenching by TOTAPOL radicals, DNP-CP-MAS at 100 K provided global sensitivity enhancements of 23 and 45 for 13C and 29Si, respectively, relative to standard CP-MAS measurements at room temperature. The effects of DNP were also ascertained by comparing with state-of-the-art two-dimensional heteronuclear 1H{13C} and 29Si{1H} correlation spectra, using, respectively, indirect detection or Carr–Purcell–Meiboom–Gill (CPMG) refocusing to boost signal acquisition. This study highlights opportunities for further improvements through the development of high-field DNP, better polarizing agents, and improved capabilities for low-temperature MAS.Show less >
Language :
Anglais
Peer reviewed article :
Oui
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
Université de Lille
CNRS
CNRS
Collections :
Research team(s) :
Propriétés magnéto structurales des matériaux (PMSM)
Submission date :
2021-06-17T14:31:21Z
2021-10-06T16:32:46Z
2021-10-06T16:32:46Z